A Comparative Study of Nanosized Gold and Copper Catalysts on Y-doped Ceria for the Water-Gas Shift Reaction

T. Tabakova, I. Ivanov, J. Sobczak, W. Lisowski, Z. Kaszkur, R. Zanella, P. Petrova, Y. Karakirova, L. Ilieva
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Abstract

The increasing demands for high-purity hydrogen for fuel-cell processing systems caused a renewed interest in the watergas shift reaction. This work aims to analyse the suitability of goldand copper-based catalysts for efficient upgrading the purity of hydrogen for small-scale applications. New catalytic materials were developed by deposition of nanosized gold or copper oxide particles on ceria doped by various amount of Y2O3 (1.0, 2.5 and 5.0 wt.%). A favourable effect of the ceria modification on the WGS activity of gold/ceria catalysts was observed. Superior CO conversion degrees (> 95 %) were achieved in the range 180-220 °C. The similarity in the catalytic activity was explained with the insignificant differences in the gold particle size among all gold-based samples. Surprisingly, copper-based catalysts exhibited decreased activity at increasing amount of Y2O3 in the composition of ceria supports. A characterization of the catalysts by N2 physisorption, XRD, HRTEM/HAADF, XPS, EPR and H2-TPR was carried out to reveal the effect of dopant amount on the WGS activity. The differences in the WGS performance were related to the catalysts reducibility, e.g. the availability of oxygen species with enhanced mobility. The analysis of structure-property-WGS activity relations proved to be a reliable tool for the improvement of catalyst performance by rational changes in the catalyst composition and structure.
纳米金与铜催化剂对y掺杂二氧化铈水气转换反应的比较研究
燃料电池处理系统对高纯度氢的需求不断增加,引起了人们对水转换反应的新兴趣。这项工作旨在分析金基和铜基催化剂在小规模应用中有效提高氢纯度的适用性。将纳米级的氧化金或氧化铜颗粒沉积在掺有不同重量的Y2O3(1.0、2.5和5.0 wt.%)的氧化铈上,开发了新的催化材料。观察到铈改性对金/铈催化剂的WGS活性有良好的影响。在180-220°C范围内,CO转化率达到了95%以上。催化活性的相似性可以用各金基样品的金粒度差异不显著来解释。令人惊讶的是,随着氧化铈载体中Y2O3含量的增加,铜基催化剂的活性降低。通过N2物理吸附、XRD、HRTEM/HAADF、XPS、EPR和H2-TPR对催化剂进行表征,揭示了掺杂量对WGS活性的影响。WGS性能的差异与催化剂的还原性有关,如氧的可用性和迁移率的提高。结构-性能- wgs活性关系的分析是通过合理改变催化剂组成和结构来改善催化剂性能的可靠工具。
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